The development of multifunctional radiation protection materials is crucial to ensure the safety of personnel and equipment in complex nuclear environments. Herein, a flexible radiation protection material integrating self-healing, thermal management, and behaviour response was prepared from Ta4C3Tx MXene, Hydrogen-terminated phenyl polysiloxane, and Polyborosiloxane through esterification, “thiol-ene click” hydrosilylation reaction using L(+)-Cysteine as a bridge. The results showed that when Ta4C3Tx MXene reached 20 wt%, the tensile strength of composite was 0.6321 MPa with the self-healing rate at 90.22 %. And the gauge factor of the material reached 25.83 at 100 % strain. This compensated for the gap between low strain and high sensitivity. Additionally, the multilayer structure of Ta4C3Tx MXene and the absorption properties of Tantalum enable the material to attenuate γ-rays through absorption and scattering mechanisms. The attenuation capability of Ta2O5 and Ta4C3Tx MXene fillers for 59.6 KeV γ-rays was compared at the same Tantalum content. When the Tantalum content reaches 23.81 wt%, the Ta4C3Tx MXene composite contains 20 wt% filler and has an attenuation coefficient of 0.757. Similarly, the Ta2O5 composite contains 22.5 wt% filler and has an attenuation coefficient of 0.734. These results are significant for improving temperature and behaviour monitoring of workers in low-temperature nuclear environments.